Abstract
AbstractTwo Pt single‐atom catalysts (SACs) of Pt‐GDY1 and Pt‐GDY2 were prepared on graphdiyne (GDY)supports. The isolated Pt atoms are dispersed on GDY through the coordination interactions between Pt atoms and alkynyl C atoms in GDY, with the formation of five‐coordinated C1‐Pt‐Cl4 species in Pt‐GDY1 and four‐coordinated C2‐Pt‐Cl2 species in Pt‐GDY2. Pt‐GDY2 shows exceptionally high catalytic activity for the hydrogen evolution reaction (HER), with a mass activity up to 3.3 and 26.9 times more active than Pt‐GDY1 and the state‐of‐the‐art commercial Pt/C catalysts, respectively. Pt‐GDY2 possesses higher total unoccupied density of states of Pt 5d orbital and close to zero value of Gibbs free energy of the hydrogen adsorption (|Δ |) at the Pt active sites, which are responsible for its excellent catalytic performance. This work can help better understand the structure–catalytic activity relationship in Pt SACs.
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